Small
·
2022
·Vol. 19
·期 2
·2205719
·
IF 15.153
Wenjun He,Rui Zhang,Da Cao,Ying Li,Jun Zhang,Qiuyan Hao,Hui Liu,Jianling Zhao,Huolin L. Xin
Exploiting active and stable non-precious metal electrocatalysts for alkaline hydrogen evolution reaction (HER) at large current density plays a key role in realizing large-scale industrial hydrogen generation. Herein, a self-supported microporous Ni(OH) x /Ni 3 S 2 heterostructure electrocatalyst on nickel foam (Ni(OH) x /Ni 3 S 2 /NF) that possesses super-hydrophilic property through an electrochemical process is rationally designed and fabricated. Benefiting from the super-hydrophilic property, microporous feature, and self-supported structure, the electrocatalyst exhibits an exceptional HER performance at large current density in 1.0 M KOH, only requiring low overpotential of 126, 193, and 238 mV to reach a current density of 100, 500, and 1000 mA cm −2 , respectively, and displaying a long-term durability up to 1000 h, which is among the state-of-the-art non-precious metal electrocatalysts. Combining hard X-rays absorption spectroscopy and first-principles calculation, it also reveals that the strong electronic coupling at the interface of the heterostructure facilitates the dissociation of H 2 O molecular, accelerating the HER kinetics in alkaline electrolyte. This work sheds a light on developing advanced non-precious metal electrocatalysts for industrial hydrogen production by means of constructing a super-hydrophilic microporous heterostructure.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yang Peng,Zhanwei Xu,Le Yu,Xucheng Li,Weiran Yang
The direct conversion of furfural (FUR) to 2-methyltetrahydrofuran (2-MTHF) was investigated over a trimetallic CuNiRe/Hβ catalyst. Under optimal reaction conditions at 240 °C under 3 MPa H 2 for 1 h, almost complete conversion of FUR and high-yield of 2-MTHF (81 %) was achieved. This is the highest yield reported for the direct conversion of FUR to 2-MTHF. HR-TEM demonstrated that the growth of Cu nanoparticles (NPs) on the surface of Hβ was inhibited after loading Ni or Re resulted in the smaller Cu particle size and better hydrogenation and hydrodeoxygenation activity. H 2 -TPR characterization exhibited that the reducibility of bimetallic and trimetallic catalysts was higher than that of monometallic catalysts·NH 3 -TPD explained that Hβ acid sites mainly contributed to FUR deoxygenation. The adsorption configurations of FUR, furfuryl alcohol (FOL) and 2-methylfuran (2-MF) on the catalyst were revealed by ATR-IR. Catalyst evaluation and control experiments proved that FUR was first hydrogenated to FOL, followed by hydrodeoxygenation to 2-MF, and finally hydrogenated to 2-MTHF catalyzed by the combination of three metals.
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MATERIALS CHEMISTRY AND PHYSICS
·
2022
·
IF 4.778
Xijun Li,Sifan Zhang,Lihua Zhu,Jun Liu,Huan Zhang,Ning Zhao,Bing Hui Chen
Herein, a series of the Pt-based bimetallic catalysts (PtM x /SBA-15) are gained by using ultrasonic incipient wetness impregnation method (M = Co, Cu, Ni or Zn). The experimental results show that the catalytic performance (including catalytic activity (turnover frequency-TOF), selectivity to crotyl alcohol) of PtCo x /SBA-15 for catalyzing crotonaldehyde selective hydrogenation is the best among PtM x /SBA-15. Additionally, the ratio of Pt/Co in the PtCo x /SBA-15 catalysts is changed to successfully synthesize PtCo/SBA-15, PtCo 2 /SBA-15, PtCo 5 /SBA-15. It demonstrates that the selectivity of the PtCo x /SBA-15 catalysts for crotonaldehyde selective hydrogenation to crotyl alcohol is significantly improved with the increase of the Co content. The PtCo 5 /SBA-15 catalyst provides 83.8% conversion of crotonaldehyde, 94.3% selectivity to crotyl alcohol and TOF of 910.5 h −1 under mild reaction conditions (3.0 MPa H 2 , 80 °C and 2.0 h). And PtCo 5 /SBA-15 has much better catalytic performance (higher catalytic activity and selectivity to crotyl alcohol) than PtCu 5 /SBA-15, PtNi 5 /SBA-15 and PtZn 5 /SBA-15. The reasons are as follows: (1) PtCo alloy forms, which is conducive to crotonaldehyde adsorption and activation; (2) there is an appropriate synergy effect between Pt and Co, greatly improving the capacity of the catalyst activating hydrogen under mild conditions; (3) the electron transfers from Co to Pt, resulting in the increase of Pt electron density and decrease of Co electron density, then the Co sites are advantageous to C O group adsorption and activation and Pt sites for H 2 adsorbing and activating; (4) with the increase of the Co proportion in PtCo x /SBA-15, the synergy effect between Pt and Co in PtCo alloy strengthens and thus increases the selectivity of C O group hydrogenation.
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 47
·22778-22785
·
IF 3.925
Xiaozhi Li,Jutao Qiao,Dan Luo,Siyi Xu,Yuefeng Liu,Hao Liu
In this study, Ni nanoparticles were grown on a silver-coated nylon yarn (SCNY) surface by electrochemical deposition to prepare SCNY@Ni. The hierarchical Ni–Ag nanostructure promoted their synergistic effect, which enhanced the electrocatalytic behavior of glucose oxidation. The test result of SCNY@Ni showed its high sensitivity (115.26 μA mM−1 cm−2 and 67.37 μA mM−1 cm−2) with a wide linear response (from 2 μM to 1 mM and from 1 mM to 22 mM) of glucose con-centration range, a low detection limit (LOD) of 2 μM, fast response time (3 s), and good selectivity for glucose determination in the presence of sucrose (SU), aceta-mino phenol (AP), D-fructose (D-Fru), ascorbic acid (AA), dopamine (DA), hydro-quinone (HQ) and uric acid (UA) as potential interference species. Also, SCNY@Ni exhibited excellent stability, repeatability, reproducibility and flexibility. It has good prospects for large-scale production.
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Chemistry-An Asian Journal
·
2022
·Vol. 17
·期 24
·e202200993
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IF 4.839
Zhijie Zhu,Xu Hu,Xingda An,Mengqi Xiao,Liang Zhang,Chaoran Li,Le He
Graphical The influence of the composition of bimetallic nanocrystals on their performance of photothermal catalytic CO 2 hydrogenation was investigated. Pd and Ni play different roles in the photothermal catalytic processes in the bimetallic system, which leads to a functional tradeoff over the stoichiometric ratio. Bimetallic nanomaterials exhibit excellent catalytic performance in photothermal CO 2 hydrogenation due to the synergistic effect between the two metal components. However, the component-performance relationship remains unclear, which hinders the design of efficient bimetallic catalysts and the investigation of catalytic reaction mechanism. Here we illustrate the influence of the composition of binary alloy on their performance of photothermal catalytic CO 2 hydrogenation by using monodispersed Pd−Ni nanocrystal as an example. Our study reveals that Ni and Pd play a significantly different role in the catalytic processes. Higher Ni component in the catalysts could lead to stronger light absorption, higher activity, and lower CO selectivity. The optimized Pd 4 Ni 1 −SiO 2 catalyst exhibited a near-unity and stable CO production rate of 230 mmol ⋅ g −1 ⋅ h −1 under 25-sun illumination. This study paves the way for the usage of bimetal in photothermal CO 2 catalysis towards more efficient solar-to-chemical energy conversions, and sheds light on some general design principles of bimetallic catalysts to balance the intrinsic properties of individual components.
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高影响因子
Catalysts
·
2022
·Vol. 12
·期 10
·1286
·
IF 4.501
Ravi Balaga,Kishore Ramineni,Xiaoqiang Zhang,Peifang Yan,Mahender Reddy Marri,Vijayanand Perupogu,Zongchao Conrad Zhang
Conversion of biomass-derived furfural (FFA) platform molecule to value-added tetrahydrofurfuryl alcohol (THFA) molecule is a sustainable route using an efficient non-noble metallic catalyst in water solvent. In this work, Ni in various loadings on mesoporous titanium dioxide (m-TiO2) was synthesized in one pot by Evaporation-Induced Self-Assembly (EISA). The synthesised catalysts were evaluated for the hydrogenation of furfural to tetrahydrofurfuryl alcohol. The catalysts were characterised using a combination of spectroscopic techniques such as XRD, H2-TPR, H2-TPD, XPS, SEM-EDX, TEM, and HR-TEM. The characterization results show that the Ni/m-TiO2materials exhibit enhanced electron-rich active sites, facilitated hydrogen spillover, uniform dispersion of small Ni particles (~5 nm), and strong metal support interaction between Ni and TiO2. Among the various Ni dopings, 7.5 wt.% Ni/m-TiO2catalyst exhibited the best performance and achieved 99.9% FFA conversion and 93.2% THFA selectivity in water solvent at 100 °C and under 2 MPa H2. Additionally, detailed kinetic studies, process parameters, the stability and reusability of the catalyst were also studied. The results demonstrated that the 7.5 wt.% Ni/m-TiO2catalyst is highly active and stable.Keywords:biomass;furfural hydrogenation;electron-rich Ni;SMSI;spillover
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Nanomaterials
·
2022
·Vol. 12
·期 17
·2968
·
IF 5.719
Siyu Long,Lingyu Zhang,Zhuoyue Liu,Huibin Jiao,Aiwen Lei,Wei Gong,Xianglin Pei
The hydrogenation products of aromatic molecules with reducible groups (such as C=C, NO2, C=O, etc.) are relatively critical intermediate compounds in fine chemicals, but how to accurately reduce only specific groups is still challenging. In this work, a bimetallic Pt-Ni/Chitin catalyst was prepared for the first time by using renewable biomass resource chitin as support. As the carrier, the chitin was constructed into porous nanofibrous microspheres through the sol-gel strategy, which was favorable for the adhesion of nano-metals and the exchange of reactive substances due to its large surface area, porous structure, and rich functional groups. Then the Pt-Ni/Chitin catalyst was applied to selective hydrogenation with the model substrate of 4-nitrostyrene. As the highly dispersed Pt-Ni NPs with abundant exposed active sites and the synergistic effect of bimetals, the Pt-Ni/Chitin catalyst could efficiently and selectively hydrogenate only NO2or C=C with yields of ~99% and TOF of 660 h−1, as well as good stability. This utilization of biomass resources to build catalyst materials would be important for the green and sustainable chemistry.Keywords:biomass chitin;Pt-Ni nanoparticles;supported catalyst;hydrogenation
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ENERGY & FUELS
·
2022
·
IF 4.654
Ziyi Liu,Mengxue Wu,Jinfu Ma
Ammonia is a very promising source of carbon-free chemical energy. However, current electrochemical technologies for ammonia use are limited by the kinetically sluggish and easily toxic catalyst surface ammonia oxidation reaction (AOR). Here, we report an AOR catalyst in which Ni, Cu, and Co are highly dispersed on single-walled carbon nanotubes (CNTs) (Ni–Cu–Co/CNT) in the form of hydroxides and hydroxyl oxides by using a one-step solvothermal method. Ni–Cu–Co/CNT, with Co doping and a support of the CNT, has shown highly efficient catalytic activity for the AOR in alkaline media. Cyclic voltammetry tests show that the catalyst has an onset potential of 0.3 V vs Ag/AgCl and a peak current of 96 mA cm–2. Density functional theory suggests that the addition of Co and a CNT leads to a lower energy barrier for the critical AOR step, which can be attributed to intermetallic synergy and metal–support interactions formed by the CNT.
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FUEL
·
2022
·
IF 8.035
Ning Zhang,Jing Wang,Wen Zhang,Yingxiu Zhao,Zemeng Dong,Zexing Wu,Guang-Rui Xu,Lei Wang
Despite considerable efforts to study direct alcohol fuel cells (DAFCs), the development of efficient bifunctional catalysts for monohydric alcohol and polyhydric alcohols remains a great challenge. This work reports the preparation of self-supported PdNi dendrites on Ni foam (self-supported PdNi DNTs/NF) with a large specific surface area by a simple self-sacrificing template and hydrothermal method. The presence of NF with enrichment of nucleation sites is crucial for the generation of self-supported PdNi DNTs. The as-obtained self-supported PdNi DNTs/NF exhibits an excellent property for ethanol and glycerol electrooxidation with the mass activity of 2375.7 mA mg cat −1 and 2451.6 mA mg cat −1 , the specific activity of 10.07 mA cm −2 and 10.84 mA cm −2 , respectively, in alkaline media, which should attribute to abundant high-index facets and low-coordinated atoms on the edge of branches. Furthermore, the PdNi DNTs/NF exhibits outstanding long-term durability in the current–time test for 7200 s with superior anti-CO poisoning performance, possessing a potential application in DAFCs.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Minjun Liu,Ying Liu,Xinru Liu,Chengcheng Chu,Ducheng Yao,Shun Mao
Metal organic framework (MOF)-derived materials normally have three-dimensional (3D) structure, while little attention has been paid to two-dimensional (2D) MOF-derived materials with high catalytic activity. Nevertheless, the underlying agglomeration and metal leaching issues of 2D MOF-derived catalysts hinder their real applications. In this work, we report a bimetallic nanocomposite (Ni-Fe-C-600-acid/GO) derived from 2D Ni-Fe-MOF and graphene oxide (GO) network. Employing Ni(0) and Fe 3 O 4 as active site, the Ni-Fe-C-600-acid/GO shows high efficiency in peroxydisulfate (PDS) activation for the removal of p-chloroaniline (PCA), and the catalyst/PCA dosage ratio (0.8) is substantially lower than those of the previous studies (3.9–156.9). The prepared catalysts demonstrate high catalytic activity over a wide pH range of 3–9 and maintain high efficiency after five cycles with good tolerance to inorganic anions. The singlet oxygen is identified as the predominant active species and relatively weak contributions from sulfate free radicals and hydroxyl radicals are confirmed. This catalysis system presents new insights in 2D MOF-derived catalysts in advanced oxidation processes .
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Bo Liu,Siming Yan,Yi He,Teng He,Yahui He,Ruxia Song,Zhifei Zhang,Hongjie Li,Jinxue Song,Zhiyuan Li
In this work, with the help of pulsed electrodeposition technology, Ni–W/ZrPP composite coatings on carbon steel surfaces were fabricated. The enhancing effects of inorganic layered alpha-zirconium phosphate (αZrP) and organic zirconium phenylphosphonate (ZrPP) on the surface morphology, microhardness, wear resistance and corrosion resistance of Ni–W coatings were also investigated. The result shows, Ni–W/ZrPP composite coating exhibits the most complete and dense surface morphology without any pinholes and generation of microcracks. Furthermore, the embedding of ZrPP also maximizes the wear and corrosion resistance of the Ni–W coating. This can be reflected by the fact that the Ni–W/ZrPP composite coating has the shallowest and narrowest wear section and the lowest average friction coefficient (0.312). In 3.5 wt.%NaCl solution, the Ni–W/ZrPP composite coating has the highest corrosion potential (E corr = −0.28 V) and the lowest corrosion current density (i corr = 2.3 μA cm −2 ), which show the best corrosion resistance. Relevant mechanistic studies have proven that embedding ZrPP with larger interlayer spacing in the coating is beneficial to promote the interlayer slip of 2D materials and to from frictional transfer films. The hydrophobic group and lamellar structure at the end of ZrPP are also contributors to build a physical barrier and prevent corrosive media from entering the coating.
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ENERGY & FUELS
·
2022
·
IF 4.654
Shumei Chen,Chao Miao,Lixing Liang,Jing Ouyang
This paper reports the synthesis and CO2 methanation performance of Ni/CeO2–ZrO2 (CZ) solid solutions assembled on different clay minerals (rectorite, attapulgite, halloysite, and kaolin). The catalytic performance of the samples was examined in temperature range 200−400 °C at normal pressures. The attapulgite (ATP) assembled Ni nps-incorporated-CZ solid solution (Ni–CZA) has the highest CO2 conversion and excellent stability. The CO2 conversion of the Ni–CZA catalyst reached up to 81.2% at 400 °C, and CH4 selectivity was nearly 100%. The catalyst assembled on ATP has excellent adsorption performance and a large specific surface area, resulting in higher Ce3+ and adsorbed oxygen content, thanks to the high content of oxygen vacancies and faster oxygen transfer speed. Mechanistic analysis shows that the H2 dissociates at the Ni site, the CO2 was decomposed into CO and O, and the ATP and CZ provide hydroxyls and oxygen vacancies, respectively, in this composite catalyst.
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